Solid state core-exciton dynamics in NaCl observed by tabletop attosecond four-wave mixing spectroscopy
Abstract
Nonlinear wave mixing in solids with ultrafast x-rays can provide insight into complex electronic dynamics of materials. Here, tabletop-based attosecond noncollinear four-wave mixing (FWM) spectroscopy using one extreme ultraviolet (XUV) pulse from high harmonic generation and two separately timed few-cycle near-infrared (NIR) pulses characterizes the dynamics of the Na+ L2,3 edge core-excitons in NaCl around 33.5 eV. An inhomogeneous distribution of core-excitons underlying the well-known doublet absorption of the Na+ Γ point core-exciton spectrum is deconvoluted by the resonance-enhanced nonlinear wave mixing spectroscopy. In addition, other dark excitonic states that are coupled to the XUV-allowed levels by the NIR pulses are characterized spectrally and temporally. Approximately <10fs coherence lifetimes of the core-exciton states are observed. Furthermore, the core-excitonic properties are discussed in the context of strong electron-hole exchange interactions, electron-electron correlation, and electron-phonon broadening. This investigation successfully indicates that tabletop attosecond FWM spectroscopies represent a viable technique for time-resolved solid state measurements.
- Authors:
-
[1];
[2];
[1];
[3];
[1];
[1];
[1]
- Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
- Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Princeton Univ., NJ (United States)
- Univ. of California, Berkeley, CA (United States)
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); US Air Force Office of Scientific Research (AFOSR); William Keck Foundation
- OSTI Identifier:
- 1845298
- Alternate Identifier(s):
- OSTI ID: 1821669
- Grant/Contract Number:
- AC02-05CH11231; FA9550-20-1-0334; FA9550-15-1-0037; FA9550-19-1-0314; 046300; 993922
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Physical Review. B
- Additional Journal Information:
- Journal Volume: 103; Journal Issue: 24; Journal ID: ISSN 2469-9950
- Publisher:
- American Physical Society (APS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; electronic structure of atoms & molecules; excitons; insulators; ionic solids; attosecond laser spectroscopy; four-wave mixing; high-harmonic generation
Citation Formats
Gaynor, James D., Fidler, Ashley P., Lin, Yen-Cheng, Chang, Hung-Tzu, Zuerch, Michael, Neumark, Daniel M., and Leone, Stephen R. Solid state core-exciton dynamics in NaCl observed by tabletop attosecond four-wave mixing spectroscopy. United States: N. p., 2021.
Web. doi:10.1103/physrevb.103.245140.
Gaynor, James D., Fidler, Ashley P., Lin, Yen-Cheng, Chang, Hung-Tzu, Zuerch, Michael, Neumark, Daniel M., & Leone, Stephen R. Solid state core-exciton dynamics in NaCl observed by tabletop attosecond four-wave mixing spectroscopy. United States. https://doi.org/10.1103/physrevb.103.245140
Gaynor, James D., Fidler, Ashley P., Lin, Yen-Cheng, Chang, Hung-Tzu, Zuerch, Michael, Neumark, Daniel M., and Leone, Stephen R. Fri .
"Solid state core-exciton dynamics in NaCl observed by tabletop attosecond four-wave mixing spectroscopy". United States. https://doi.org/10.1103/physrevb.103.245140. https://www.osti.gov/servlets/purl/1845298.
@article{osti_1845298,
title = {Solid state core-exciton dynamics in NaCl observed by tabletop attosecond four-wave mixing spectroscopy},
author = {Gaynor, James D. and Fidler, Ashley P. and Lin, Yen-Cheng and Chang, Hung-Tzu and Zuerch, Michael and Neumark, Daniel M. and Leone, Stephen R.},
abstractNote = {Nonlinear wave mixing in solids with ultrafast x-rays can provide insight into complex electronic dynamics of materials. Here, tabletop-based attosecond noncollinear four-wave mixing (FWM) spectroscopy using one extreme ultraviolet (XUV) pulse from high harmonic generation and two separately timed few-cycle near-infrared (NIR) pulses characterizes the dynamics of the Na+ L2,3 edge core-excitons in NaCl around 33.5 eV. An inhomogeneous distribution of core-excitons underlying the well-known doublet absorption of the Na+ Γ point core-exciton spectrum is deconvoluted by the resonance-enhanced nonlinear wave mixing spectroscopy. In addition, other dark excitonic states that are coupled to the XUV-allowed levels by the NIR pulses are characterized spectrally and temporally. Approximately <10fs coherence lifetimes of the core-exciton states are observed. Furthermore, the core-excitonic properties are discussed in the context of strong electron-hole exchange interactions, electron-electron correlation, and electron-phonon broadening. This investigation successfully indicates that tabletop attosecond FWM spectroscopies represent a viable technique for time-resolved solid state measurements.},
doi = {10.1103/physrevb.103.245140},
journal = {Physical Review. B},
number = 24,
volume = 103,
place = {United States},
year = {Fri Jun 25 00:00:00 EDT 2021},
month = {Fri Jun 25 00:00:00 EDT 2021}
}
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